Dissolution experiments of commercial PWR (52 MWd/kgU) and BWR (53 MWd/kgU) spent nuclear fuel cladded segments in bicarbonate water under oxidizing conditions. Experimental determination of matrix and instant release fraction

摘要

The denominated instant release fraction (IRF) is considered in performance assessment (PA) exercises to govern the dose that could arise from the repository. A conservative definition of IRF comprises the total inventory of radionuclides located in the gap, fractures, and the grain boundaries and, if present, in the high burn-up structure (HBS). The values calculated from this theoretical approach correspond to an upper limit that likely does not correspond to what it will be expected to be instantaneously released in the real system. Trying to ascertain this IRF from an experimental point of view, static leaching experiments have been carried out with two commercial UO2 spent nuclear fuels (SNF): one from a pressurized water reactor (PWR), labelled PWR, with an average burn-up (BU) of 52 MWd/kgU and fission gas release (FGR) of 23.1%, and one from a boiling water reactor (BWR), labelled BWR, with an average BU of and 53 MWd/kgU and FGR of 3.9%.; One sample of each SNF, consisting of fuel and cladding, has been leached in bicarbonate water during one year under oxidizing conditions at room temperature (25 +/- 5) degrees C. The behaviour of the concentration measured in solution can be divided in two according to the release rate. All radionuclides presented an initial release rate that after some days levels down to a slower second one, which remains constant until the end of the experiment. Cumulative fraction of inventory in aqueous phase (FIAPc) values has been calculated. Results show faster release in the case of the PWR SNF. In both cases Np, Pu, Am, Cm, Y, Tc, La and Nd dissolve congruently with U, while dissolution of Zr, Ru and Rh is slower. Rb, Sr, Cs and Mo, dissolve faster than U. The IRF of Cs at 10 and 200 days has been calculated, being (3.10 +/- 0.62) and (3.66 +/- 0.73) for PWR fuel, and (035 +/- 0.07) and (0.51 +/- 0.10) for BWR fuel. (C) 2015 Elsevier B.V. All rights reserved.